Energy landscapes and functions of supramolecular systems

Tantakitti, Faifan; Boekhoven, Job; Wang, Xin; Kazantsev, Roman V.; Yu, Tao; Li, Jiahe; Zhuang, Ellen; Zandi, Roya; Ortony, Julia H.; Newcomb, Christina J.; Palmer, Liam C.; Shekhawat, Gajendra S.; Cruz, Mónica Olvera de la; Schatz, George C.; Stupp, Samuel I.

doi:10.1038/nmat4538

Cited by 351 publications

(459 citation statements)

References 36 publications

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“…S1A). Upon annealing, certain PA nanofibers elongate effectively to "infinite" length as they reach their thermodynamically stable state, according to PA concentration and ionic strength (28). We have confirmed this for three previously described PAs by imaging them by cryogenic transmission electron microscopy (CryoTEM) before and after annealing.…”

Section: Resultssupporting

confidence: 77%

Injectable biomimetic liquid crystalline scaffolds enhance muscle stem cell transplantation

Sleep

Cosgrove

McClendon

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

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Muscle stem cells are a potent cell population dedicated to efficacious skeletal muscle regeneration, but their therapeutic utility is currently limited by mode of delivery. We developed a cell delivery strategy based on a supramolecular liquid crystal formed by peptide amphiphiles (PAs) that encapsulates cells and growth factors within a muscle-like unidirectionally ordered environment of nanofibers. The stiffness of the PA scaffolds, dependent on amino acid sequence, was found to determine the macroscopic degree of cell alignment templated by the nanofibers in vitro. Furthermore, these PA scaffolds support myogenic progenitor cell survival and proliferation and they can be optimized to induce cell differentiation and maturation. We engineered an in vivo delivery system to assemble scaffolds by injection of a PA solution that enabled coalignment of scaffold nanofibers with endogenous myofibers. These scaffolds locally retained growth factors, displayed degradation rates matching the time course of muscle tissue regeneration, and markedly enhanced the engraftment of muscle stem cells in injured and noninjured muscles in mice.biomaterials | scaffold | muscle stem cell | cell delivery | muscle regeneration

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Section: Resultssupporting

confidence: 77%

Injectable biomimetic liquid crystalline scaffolds enhance muscle stem cell transplantation

Sleep

Cosgrove

McClendon

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

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“…For example, the ability to pass a gel through a needle and have quick recoverability has been linked to the gel's microstructure. 95 Further changes in the properties of a peptide amphiphile system have been reported recently, 57 where different lengths of selfassembled fibers were prepared by varying the assembly process via dilution and annealing steps. Pre-myoblasts were grown in media containing either short or long fibers, with significantly higher cell death observed in the presence of the shorter fibers.…”

Section: Process Of Assemblymentioning

confidence: 92%

“…To some degree, these have been covered in previous reviews, [55][56][57][58][59][60] but as the field is developing rapidly we believe that a further critical analysis is warranted. Both of these areas also allow us to further discuss the assembly process.…”

Section: Introductionmentioning

confidence: 99%

Low-Molecular-Weight Gels: The State of the Art

Draper

Adams

2017

Chem

485

447

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Low-molecular-weight gels are currently a hugely important class of materials that are attracting significant interest. These gels are formed when small molecules self-assemble into one-dimensional structures that entangle and cross-link to form a network that is capable of immobilizing the solvent. Here, we critically discuss the current state of the art and highlight two key areas where we believe there is significant untapped potential. The first is the observation that the properties of the gels are highly process dependent, which means that it is possible to access materials with very different properties from a single gelator. Second, using multiple gelators offers the opportunity to prepare materials with a high degree of information content and with a wider range of properties. We aim to spark thought and discussion on these aspects. INTRODUCTIONLow-molecular-weight gels (LMWGs), or supramolecular gels, are a fascinating and useful class of material. The gels arise from the self-assembly of small molecules into long, anisotropic structures, most commonly fibers. [1][2][3][4][5] At a sufficiently high concentration, these fibers entangle or otherwise form cross-links, leading to the network that is able to immobilize the solvent through surface tension and capillary forces. 1,2 These gels differ from permanently covalently cross-linked polymer gels because the cross-linking can be reversed by the input of energy, for example, by heating. 6 LMWGs have been around for many years but are receiving considerable current interest. 4 They are also used in industrial products, 7 although this seems rarely discussed in the academic literature.In addition to the industrial applications, many recent advances and uses are being described. [8][9][10][11][12] The specific self-assembly leading to gel formation can be exploited. For example, the fiber formation is a result of molecular stacking, meaning that the self-assembly leads to aggregates that can be suitable for optoelectronic applications. 13,14 The ready reversibility of gelation can be exploited, for example, to release cells from gels on demand in a manner that does not lead to cell death. 15 Ready gel formation by a simple trigger can also be used to allow easy and efficient gel loading. [16][17][18] Unsurprisingly, therefore, there is significant interest in these materials ( Figure 1). This is a fascinating area and in many ways holds attention because of the difficulties in probing and understanding the gels. The gels arise from assembly across many length scales, and understanding all of these is difficult. At the molecular level, the molecules must interact in a manner that leads to the formation of suitable aggregates that can eventually entangle. Thus, one-dimensional growth must be favored. From this perspective, it is very frustrating that it is often extremely difficult to predict whether a molecule will form a gel or not; indeed, gelation has been described as an empirical science. 4 Structurally similar small molecules can exhibitThe Bigger Pict...

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“…[3][4][5][6][7] Directing the noncovalent interactions allows controlling the properties of the resulting supramolecular constructs. [8][9][10][11][12] In addition, the proper choice of assembly protocols helps in tuning the properties of biomaterials 13 or improves the performance of organic semiconductors. 14 Thus, the chemical composition alone is often insufficient to achieve the best performance of complex supramolecular assemblies, among which DNA-based materials take a prominent role.…”

Section: Introductionmentioning

confidence: 99%

Pathway Diversity in the Self-Assembly of DNA-Derived Bioconjugates

Vyborna

Vybornyi²,

Häner

2016

Bioconjugate Chem.

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The pathway diversity of the self-assembly of amphiphilic DNA-pyrene conjugates is described.The hydrophobic pyrene units drive the self-assembly of the anionic oligomers in an aqueous environment into ribbon-shaped, DNA-grafted supramolecular polymers. Isothermal mixing of two types of sorted ribbons, each of which contains only one kind of two complementary oligonucleotides, results in the formation of tight networks. Thermal disassembly of these kinetically trapped networks and subsequent re-assembly of the liberated components leads to mixed supramolecular polymers, which now contain both types of oligonucleotides. The scrambling of the oligonucleotides prevents the interaction between ribbons and, thus, network formation. The results show that a high local density of DNA strands in linear arrays favors hybridization among sorted polymers, whereas hybridization among mixed arrays is prevented. The lack of DNA hybridization among mixed ribbons is ascribed to the electrostatic repulsion between identical, hence non-complementary, oligonucleotides. The findings highlight the importance of kinetically trapped states on the structural and functional properties of supramolecular polymers containing orthogonal self-assembly motifs.

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Energy landscapes and functions of supramolecular systems

Cited by 351 publications

References 36 publications

Injectable biomimetic liquid crystalline scaffolds enhance muscle stem cell transplantation

Injectable biomimetic liquid crystalline scaffolds enhance muscle stem cell transplantation

Low-Molecular-Weight Gels: The State of the Art

Pathway Diversity in the Self-Assembly of DNA-Derived Bioconjugates

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